期刊
CCS CHEMISTRY
卷 5, 期 7, 页码 1653-1662出版社
CHINESE CHEMICAL SOC
DOI: 10.31635/ccschem.022.202202189
关键词
graphdiyne; donor-acceptor interface; incomplete charge transfer; high selectivity; ammo-nia production
Efficient production of ammonia by reducing nitrates at room temperature and ambient pressure is a promising alternative to the Haber-Bosch process that can effectively overcome water pollution issues. The construction of a sp-carbon-metal-carbon interface greatly enhances charge transfer ability and electrical conductivity, leading to high selectivity, activity, and stability in the catalytic system.
The efficient production of ammonia by reducing nitrates at room temperature and ambient pressure is a promising alternative to the Haber-Bosch process and can effectively overcome the attendant water pollution issues. Herein, a new idea has been realized for rational and selective construction of the sp-carbon-metal- carbon interface, comprised of electronic-donating triple bonds in graphdiyne and electron-withdrawing iron carbides, for a highly efficient nitrate reduction reaction. The as-prepared sp-carbon-metal-carbon in-terfacial structures greatly increase the charge transfer ability and electrical conductivity of the system. The proposed concept of incomplete charge transfer has demonstrated significantly high selectivity, activity, and stability in catalytic system. The catalyst exhibits high Faradaic efficiency of over >95% and a NH3 yield rate up to 205.5 mu molNH 3 cm-2 h-1 in dilute nitrate conditions without any contaminant.
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